Schottky Defects Suppress Nonradiative Recombination in CH3NH3PbI3 through Charge Localization

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters Pub Date : 2024-12-23 DOI:10.1021/acs.jpclett.4c03313

Lu Qiao, Andrey S. Vasenko, Evgueni V. Chulkov, Run Long

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Abstract

Hybrid lead halide perovskites are promising materials for photovoltaic applications due to their exceptional optoelectronic properties. Here, we investigate the impact of Schottky defects─specifically PbI₂(V_PbI₂) and CH₃NH₃I (V_MAI) vacancies─on nonradiative recombination in CH₃NH₃PbI₃ using time-dependent density functional theory and nonadiabatic (NA) molecular dynamics. Our results reveal that Schottky defects do not alter the fundamental bandgap or introduce trap states but instead distort the surrounding lattice, localizing the hole distribution. This reduces the spatial overlap of electron and hole wave functions, weakening NA coupling and increasing intensitieis of high-intensity phonon modes that accelerate dephasing. Consequently, nonradiative recombination lifetimes extend to 2.1 and 2.6 ns for V_PbI₂ and V_MAI, respectively─over double that of pristine CH₃NH₃PbI₃. This work demonstrates the potential of Schottky defects to enhance perovskite solar cell performance by suppressing nonradiative recombination.

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来源期刊

The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY

CiteScore

9.60

自引率

7.00%

发文量

1519

审稿时长

1.6 months

期刊介绍： The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.